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Belousov–Zhabotinsky (BZ) reactions have been used to investigate periodic spatial patterns due to the oscillatory nature of the reaction. However, these systems have not been confined, nor controlled, in macro‐scaled architectures, making it hard to translate observations to natural behavior. Here, a poly(electrolyte) complex is designed that can be ionically or covalently reinforced to construct 3D geometries with additive manufacturing techniques. Printed geometries varied in shape, size, and angle to investigate spatiotemporal pattern formation in 3D. Size variations correlated to trends in oscillating pattern frequencies, demonstrating a geometry effect on spatial alterations. Overall, the combination of 3D printing techniques with self‐oscillating chemical reactions allows to model, study, and further understand macro‐scale patterns observed in nature. The proposed approach can be used to design smart structure to replicate biological oscillators such as cardiac arrhythmias, neuron signaling, and camouflage skin patterns.

Printing techniques using nanomaterials have emerged as a versatile tool for fast prototyping and potentially large‐scale manufacturing of functional devices. Surfactants play a significant role in many printing processes due to their ability to reduce interfacial tension between ink solvents and nanoparticles and thus improve ink colloidal stability. Here, a colloidal graphene quantum dot (GQD)‐based nanosurfactant is reported to stabilize various types of 2D materials in aqueous inks. In particular, a graphene ink with superior colloidal stability is demonstrated by GQD nanosurfactants via the π–π stacking interaction, leading to the printing of multiple high‐resolution patterns on various substrates using a single printing pass. It is found that nanosurfactants can significantly improve the mechanical stability of the printed graphene films compared with those of conventional molecular surfactant, as evidenced by 100 taping, 100 scratching, and 1000 bending cycles. Additionally, the printed composite film exhibits improved photoconductance using UV light with 400 nm wavelength, arising from excitation across the nanosurfactant bandgap. Taking advantage of the 3D conformal aerosol jet printing technique, a series of UV sensors of heterogeneous structures are directly printed on 2D flat and 3D spherical substrates, demonstrating the potential of manufacturing geometrically versatile devices based on nanosurfactant inks.